Laser-Induced Fluorescence Measurements and Kinetic Analysis of Si Atom Formation in a Rotating Disk Chemical Vapor Deposition Reactor

Ho, Pauline; Coltrin, Michael E.; Breiland, William G.

doi:10.1021/j100091a032

Cited by 134 publications

(161 citation statements)

References 8 publications

(9 reference statements)

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“…As seen above, the competing processes for decomposition of Si 2 H n Cl 4-n are elimination of a silicon atom or decomposition to two silylenes: or The endothermicity of the first channel (eq d1) remains relatively constant with chlorine substitution (47-50 kcal/mol). However, as seen in Table 1, the endothermicity of the second reaction (eq d2) decreases strongly with chlorine substitution, from 61 kcal/mol for Si 2 H 4 f 2SiH 2 to only 23 kcal/mol for Si 2 Cl 4 f 2SiCl 2 . This large change in enthalpy of reaction can be attributed to the substantial increase in stability in going from SiH 2 to SiHCl to SiCl 2 , the products of the second reaction path.…”

Section: Mechanismmentioning

confidence: 91%

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On the Mechanism of Homogeneous Decomposition of the Chlorinated Silanes. Chain Reactions Propagated by Divalent Silicon Species

Swihart

Carr

1998

J. Phys. Chem. A

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A mechanism for the homogeneous gas-phase decomposition of SiHCl 3 , SiH 2 Cl 2 , and SiH 3 Cl in hydrogen is derived from the results of ab initio molecular-orbital studies. It consists of 39 reversible elementary reactions among 25 species, including pressure-dependent unimolecular decomposition of the chlorinated silanes and secondary chemistry due to reactions of SiH 2 , SiHCl, and SiCl 2 with one another and with the chlorinated silanes. Rate parameters in the mechanism have been calculated based on results of ab initio studies using transition-state theory and unimolecular rate theories. This allows us to construct a reasonably complete mechanism that provides qualitative explanations for several features of dichlorosilane decomposition that have been presented in the literature, including observations on the presence and concentrations of SiCl 2 , SiHCl, and Si atoms. Several chain reactions in which the chain carriers are divalent silicon species have been identified.

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Section: Mechanismmentioning

confidence: 91%

“…Silane decomposition mechanisms are understood in more detail and have been presented and discussed elsewhere. [1][2][3] Additional chemical species and reactions would be required to describe SiCl 4 decomposition.…”

Section: Introductionmentioning

confidence: 99%

On the Mechanism of Homogeneous Decomposition of the Chlorinated Silanes. Chain Reactions Propagated by Divalent Silicon Species

Swihart

Carr

1998

J. Phys. Chem. A

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“…As a base reaction mechanism, we used the reactions and rate parameters presented by Ho et al 58 for reactions among species containing one or two silicon atoms (Si, SiH 2 , SiH 4 , Si 2 H 4 A, Si 2 H 4 B, Si 2 H 6 ). This mechanism explicitly treats the pressure dependence of the unimolecular decomposition and recombination reactions.…”

Section: Clustering Reaction Mechanism and Kineticsmentioning

confidence: 99%

“…In particular, Breiland, Coltrin, Ho, and co-workers at Sandia National Laboratories have made extensive comparisons of mathematical models and experimental measurements of silicon growth rates and reactive species concentration profiles. [1][2][3][4][5][6][7] There is also a substantial body of work on the kinetics of gas-phase reactions of small silicon hydrides. [8][9][10][11][12][13][14][15][16][17][18][19][20][21][22][23][24][25][26] On the basis of this body of research, models of thermal CVD of silicon from silane can now predict film growth rates and precursor utilization with reasonable accuracy and reliability, at least under conditions where particle formation is negligible.…”

Section: Introductionmentioning

confidence: 99%

Thermochemistry and Kinetics of Silicon Hydride Cluster Formation during Thermal Decomposition of Silane

1998

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Product contamination by particles nucleated within the processing environment often limits the deposition rate during chemical vapor deposition processes. A fundamental understanding of how these particles nucleate could allow higher growth rates while minimizing particle contamination. Here we present an extensive chemical kinetic mechanism for silicon hydride cluster formation during silane pyrolysis. This mechanism includes detailed chemical information about the relative stability and reactivity of different possible silicon hydride clusters. It provides a means of calculating a particle nucleation rate that can be used as the nucleation source term in aerosol dynamics models that predict particle formation, growth, and transport. A group additivity method was developed to estimate thermochemical properties of the silicon hydride clusters. Reactivity rules for the silicon hydride clusters were proposed based on the group additivity estimates for the reaction thermochemistry and the analogous reactions of smaller silicon hydrides. These rules were used to generate a reaction mechanism consisting of reversible reactions among silicon hydrides containing up to 10 silicon atoms and irreversible formation of silicon hydrides containing 11-20 silicon atoms. The resulting mechanism was used in kinetic simulations of clustering during silane pyrolysis in the absence of any surface reactions. Results of those simulations are presented, along with reaction path analyses in which key reaction paths and rate-limiting steps are identified and discussed.

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“…Thu s, this configura tion allows for highly uniform chemical vapor depositio n (Hitchman et al 1977 ;Pollard and Newman 1980). Due to its simple configuration and well-define d flow field, numerous numerical studies have bee n performed for both reacting and nonreacting flows (Coltrin et al 1989;Breiland and Evans 1991 ;Jensen and Einset 1991 ;Ho et al 1994). By employing a von Karman similarity transform , the equations describing the threedimensional spiral fluid motion ca n be reduc ed to a system of ordinary differenti al equations that only depend on the axia l coordinate.…”

Section: Introductionmentioning

confidence: 99%

A Sectional Model for Investigating Microcontamination in a Rotating Disk CVD Reactor

Sun

Axelbaum

Davis

2004

Aerosol Science and Technology

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A sectional model is employed to study the aerosol dynamics in a rotating disk CVD reactor. The aerosol model is implemented into a numerical code that employs detailed chemistry and transport and a one-dimensional similar ity transform to simulate this system. The numerical results are compared to experimental data where condition s are such that particles are formed from gas-phase reactions. A thin particle layer is reproduced and the thickness is accurately determined. The location of the layer is predicted within 5 %. The thin layer is a consequence of the particle stagnation region that develop s due to convection towards the disk being opposed by a particle the rmophoretic velocity away from the disk. The effect of sticking coefficient is examined , and it is shown that with a small sticking coefficient a smaller mean particle size and broader particle layer is obtained. It is also found that particle layer s are driven farther awa y from the disk when the temperature of the disk is higher or the cha mber pre ssure is lower, both of which result in higher thermophoretic velocities for the particles. The thickness of th e particle layer is found to be insen sitive to pressure. The sectional model also reveals that the particle size distributions are bimodal throughout most of the particle layer. Thi s is a result of the broad region s for nucleation and surface growth as well as the opposing convective and thermophoretic velocitie s.

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Laser-Induced Fluorescence Measurements and Kinetic Analysis of Si Atom Formation in a Rotating Disk Chemical Vapor Deposition Reactor

Cited by 134 publications

References 8 publications

On the Mechanism of Homogeneous Decomposition of the Chlorinated Silanes. Chain Reactions Propagated by Divalent Silicon Species

On the Mechanism of Homogeneous Decomposition of the Chlorinated Silanes. Chain Reactions Propagated by Divalent Silicon Species

Thermochemistry and Kinetics of Silicon Hydride Cluster Formation during Thermal Decomposition of Silane

A Sectional Model for Investigating Microcontamination in a Rotating Disk CVD Reactor

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